Samandriel manifested in a vessel around the time one of The Word of God is being auctioned. Before the auction, he approached Dean and asked him what had happened to Castiel. Dean, however, was unable to give him a straight answer. During the auction, he bid against Crowley for the tablet. Alfie's offers included the Mona Lisa and Vatican City. Crowley's counteroffers included the "real" Mona Lisa (in which Crowley claims she's topless), Alaska, and the moon. When Mrs. Tran offered her soul in exchange for the tablet and her son, the prophet Kevin Tran, Alfie was impressed and deeply moved by her courage. After the auction was over, he offered her Heaven's protection for her son. Mrs. Tran declined, however, pointing out that the last time angels tried to protect Kevin, they were killed and Kevin went missing for a year.

Samandriel is tortured by Crowley.

Later, Samandriel was captured by the King of Hell Crowley, who tortures him for information on the succeeding prophets. Crowley used an angel blade to inflict damage on Samandriel, who eventually gave up the identity of several next-in-line prophets. When he told Crowley the next generation of prophets isn't born yet, the demon stopped the torture, albeit without urgency.

He was tortured while in custody of demons. His angelic link was disabled by a screw bored into his forehead. When he removed the screw by telekinesis to send a distress signal, his demon captors sought to sever his link more effectively. Naomi then picked up his distress call and sent Castiel to save the captured angel. Castiel in turn also enlisted the help of the Winchesters and Kevin.

Samandriel revealing informations about the angels to Crowley.

Meanwhile, when the demons began to use more screws to disable the angelic link, Samandriel inadverdently began to speak in Enochian. This caught the attention of Crowley, who was interested in finding out information from the angels. The angel's agony also caused disturbances in the surrounding area, such as a bush being lit with flames. According to Crowley, the torture has tapped into Samandriel's "operating system" and he has reverted to his "factory settings." Just before Samandriel was freed by Castiel, Crowley managed to extract information from Samandriel that a tablet on angels also exists. Samandriel didn't want Castiel to bring him to Heaven because the former believed he had betrayed Heaven by revealing secrets that were unknown even to him. He was surprised that Castiel does not know Naomi and realized that he was being controlled by her. Samandriel indicates that he was once controlled as well.

Samandriel is killed by Castiel.

Samandriel's confession of what he revealed to Crowley prompted Naomi to deem him a traitor for revealing what any angel would die to protect. She ordered the assassination of Samandriel, to protect the secrets of Heaven and the angels and Castiel, unable to go against Naomi's orders, stabbed Samandriel with an Angel Blade, killing him.

His remains were brought to Heaven by Castiel under Naomi's orders, so she could find out how much information Crowley was able to extract. Castiel was left horrified by his death, though Naomi calls him a hero for it. Samandriel's death and Castiel's explanation under Naomi's control attracted the Winchesters' suspicions.

Samandriel appears to hold humans in higher respect than most other angels. This may be due to his admiration for Castiel.

Crowley's torture of Samandriel ends up being the inspiration for Dean and Castiel's plan to reach Sam so he can expel Gadreel from his body. Like Samandriel, Gadreel also has his "factory settings" activated by Crowley.